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Title: Extended Leach Testing of Simulated LAW Cast Stone Monoliths

Abstract

This revision to the original report adds two longer term leach sets of data to the report and provides more discussion and graphics on how to interpret the results from long-term laboratory leach tests. The leach tests were performed at Pacific Northwest National Laboratory (PNNL) for Washington River Protection Solutions (WRPS) to evaluate the release of key constituents from monoliths of Cast Stone prepared with four simulated low-activity waste (LAW) liquid waste streams.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1365453
Report Number(s):
PNNL-24297 Rev 1
830403000
DOE Contract Number:
AC05-76RL01830
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES

Citation Formats

Serne, R. Jeffrey, Lanigan, David C., Westsik, Joseph H., Williams, Benjamin D., Jung, H. B., and Wang, Guohui. Extended Leach Testing of Simulated LAW Cast Stone Monoliths. United States: N. p., 2016. Web. doi:10.2172/1365453.
Serne, R. Jeffrey, Lanigan, David C., Westsik, Joseph H., Williams, Benjamin D., Jung, H. B., & Wang, Guohui. Extended Leach Testing of Simulated LAW Cast Stone Monoliths. United States. doi:10.2172/1365453.
Serne, R. Jeffrey, Lanigan, David C., Westsik, Joseph H., Williams, Benjamin D., Jung, H. B., and Wang, Guohui. 2016. "Extended Leach Testing of Simulated LAW Cast Stone Monoliths". United States. doi:10.2172/1365453. https://www.osti.gov/servlets/purl/1365453.
@article{osti_1365453,
title = {Extended Leach Testing of Simulated LAW Cast Stone Monoliths},
author = {Serne, R. Jeffrey and Lanigan, David C. and Westsik, Joseph H. and Williams, Benjamin D. and Jung, H. B. and Wang, Guohui},
abstractNote = {This revision to the original report adds two longer term leach sets of data to the report and provides more discussion and graphics on how to interpret the results from long-term laboratory leach tests. The leach tests were performed at Pacific Northwest National Laboratory (PNNL) for Washington River Protection Solutions (WRPS) to evaluate the release of key constituents from monoliths of Cast Stone prepared with four simulated low-activity waste (LAW) liquid waste streams.},
doi = {10.2172/1365453},
journal = {},
number = ,
volume = ,
place = {United States},
year = 2016,
month = 8
}

Technical Report:

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  • This report describes the results from long-term laboratory leach tests performed at Pacific Northwest National Laboratory (PNNL) for Washington River Protection Solutions (WRPS) to evaluate the release of key constituents from monoliths of Cast Stone prepared with four simulated low-activity waste (LAW) liquid waste streams. Specific objectives of the Cast Stone long-term leach tests described in this report focused on four activities: 1. Extending the leaching times for selected ongoing EPA-1315 tests on monoliths made with LAW simulants beyond the conventional 63-day time period up to 609 days reported herein (with some tests continuing that will be documented later) inmore » an effort to evaluate long-term leaching properties of Cast Stone to support future performance assessment activities. 2. Starting new EPA-1315 leach tests on archived Cast Stone monoliths made with four LAW simulants using two leachants (deionized water [DIW] and simulated Hanford Integrated Disposal Facility (IDF) Site vadose zone pore water [VZP]). 3. Evaluating the impacts of varying the iodide loading (starting iodide concentrations) in one LAW simulant (7.8 M Na Hanford Tank Waste Operations Simulator (HTWOS) Average) by manufacturing new Cast Stone monoliths and repeating the EPA-1315 leach tests using DIW and the VZP leachants. 4. Evaluating the impacts of using a non-pertechnetate form of Tc that is present in some Hanford tanks. In this activity one LAW simulant (7.8 M Na HTWOS Average) was spiked with a Tc(I)-tricarbonyl gluconate species and then solidified into Cast Stone monoliths. Cured monoliths were leached using the EPA-1315 leach protocol with DIW and VZP. The leach results for the Tc-Gluconate Cast Stone monoliths were compared to Cast Stone monoliths pertechnetate.« less
  • This report describes the results from the solid phase characterization of six Cast Stone monoliths from the extended leach tests recently reported on (Serne et al. 2016),that were selected for characterization using multiple state-of-the-art approaches. The Cast Stone samples investigated were leached for > 590 d in the EPA Method 1315 test then archived for > 390 d in their final leachate. After reporting the long term leach behavior of the monoliths (containing radioactive 99Tc and stable 127I spikes and for original Westsik et al. 2013 fabricated monoliths, 238U), it was suggested that physical changes to the waste forms andmore » a depleting inventory of contaminants of potential concern may mean that effective diffusivity calculations past 63 d should not be used to accurately represent long-term waste form behavior. These novel investigations, in both length of leaching time and application of solid state techniques, provide an initial arsenal of techniques which can be utilized to perform such Cast Stone solid phase characterization work, which in turn can support upcoming performance assessment maintenance. The work was performed at Pacific Northwest National Laboratory (PNNL) for Washington River Protection Solutions (WRPS) to characterize several properties of the long- term leached Cast Stone monolith samples.« less
  • Cast Stone is undergoing evaluation as the supplemental treatment technology for Hanford’s (Washington) high activity waste (HAW) and low activity waste (LAW). This report will only cover the LAW Cast Stone. The programs used for this simulated Cast Stone were gradient density change, compressive strength, and salt waste form phase identification. Gradient density changes show a favorable outcome by showing uniformity even though it was hypothesized differently. Compressive strength exceeded the minimum strength required by Hanford and greater compressive strength increase seen between the uses of different salt solution The salt waste form phase is still an ongoing process asmore » this time and could not be concluded.« less
  • Laboratory testing and technical evaluation activities on Containerized Cast Stone (CCS) were conducted under the Scope of Work (SOW) contained in CH2M HILL Hanford Group, Inc. (CHG) Contract No. 18548 (CHG 2003a). This report presents the results of testing and demonstration activities discussed in SOW Section 3.1, Task I--''Process Development Testing'', and described in greater detail in the ''Containerized Grout--Phase I Testing and Demonstration Plan'' (CHG, 2003b). CHG (2003b) divided the CCS testing and evaluation activities into six categories, as follows: (1) A short set of tests with simulant to select a preferred dry reagent formulation (DRF), determine allowable liquidmore » addition levels, and confirm the Part 2 test matrix. (2) Waste form performance testing on cast stone made from the preferred DRF and a backup DRF, as selected in Part I, and using low activity waste (LAW) simulant. (3) Waste form performance testing on cast stone made from the preferred DRF using radioactive LAW. (4) Waste form validation testing on a selected nominal cast stone formulation using the preferred DRF and LAW simulant. (5) Engineering evaluations of explosive/toxic gas evolution, including hydrogen, from the cast stone product. (6) Technetium ''getter'' testing with cast stone made with LAW simulant and with radioactive LAW. In addition, nitrate leaching observations were drawn from nitrate leachability data obtained in the course of the Parts 2 and 3 waste form performance testing. The nitrate leachability index results are presented along with other data from the applicable activity categories.« less
  • To support the selection of a waste form for the liquid secondary wastes from WTP, Washington River Protection Solutions has initiated secondary-waste-form testing work at Pacific Northwest National Laboratory (PNNL). In anticipation of a down-selection process for a waste form for the Solidification Treatment Unit to be added to the ETF, PNNL is conducting tests on four candidate waste forms to evaluate their ability to meet potential waste acceptance criteria for immobilized secondary wastes that would be placed in the IDF. All three waste forms demonstrated compressive strengths above the minimum 3.45 MPa (500 psi) set as a target formore » cement-based waste forms. Further, none of the waste forms showed any significant degradation in compressive strength after undergoing thermal cycling (30 cycles in a 10 day period) between -40 C and 60 C or water immersion for 90 days. The three leach test methods are intended to measure the diffusion rates of contaminants from the waste forms. Results are reported in terms of diffusion coefficients and a leachability index (LI) calculated based on the diffusion coefficients. A smaller diffusion coefficient and a larger LI are desired. The NRC, in its Waste Form Technical Position (NRC 1991), provides recommendations and guidance regarding methods to demonstrate waste stability for land disposal of radioactive waste. Included is a recommendation to conduct leach tests using the ANS 16.1 method. The resulting leachability index (LI) should be greater than 6.0. For Hanford secondary wastes, the LI > 6.0 criterion applies to sodium leached from the waste form. For technetium and iodine, higher targets of LI > 9 for Tc and LI > 11 for iodine have been set based on early waste-disposal risk and performance assessment analyses. The results of these three leach tests conducted for a total time between 11days (ASTM C1308) to 90 days (ANS 16.1) showed: (1) Technetium diffusivity: ANSI/ANS 16.1, ASTM C1308, and EPA 1315 tests indicated that all the waste forms had leachability indices better than the target LI > 9 for technetium; (2) Rhenium diffusivity: Cast Stone 2M specimens, when tested using EPA 1315 protocol, had leachability indices better than the target LI > 9 for technetium based on rhenium as a surrogate for technetium. All other waste forms tested by ANSI/ANS 16.1, ASTM C1308, and EPA 1315 test methods had leachability indices that were below the target LI > 9 for Tc based on rhenium release. These studies indicated that use of Re(VII) as a surrogate for 99Tc(VII) in low temperature secondary waste forms containing reductants will provide overestimated diffusivity values for 99Tc. Therefore, it is not appropriate to use Re as a surrogate 99Tc in future low temperature waste form studies. (3) Iodine diffusivity: ANSI/ANS 16.1, ASTM C1308, and EPA 1315 tests indicated that the three waste forms had leachability indices that were below the target LI > 11 for iodine. Therefore, it may be necessary to use a more effective sequestering material than silver zeolite used in two of the waste forms (Ceramicrete and DuraLith); (4) Sodium diffusivity: All the waste form specimens tested by the three leach methods (ANSI/ANS 16.1, ASTM C1308, and EPA 1315) exceeded the target LI value of 6; (5) All three leach methods (ANS 16.1, ASTM C1308 and EPA 1315) provided similar 99Tc diffusivity values for both short-time transient diffusivity effects as well as long-term ({approx}90 days) steady diffusivity from each of the three tested waste forms (Cast Stone 2M, Ceramicrete and DuraLith). Therefore, any one of the three methods can be used to determine the contaminant diffusivities from a selected waste form.« less